Abstract:Resonant energy transfer, energy transfer upconversion, and energy pooling are considered within optical cavities to elucidate the relationship between exciton dynamics and donor/acceptor separation distance. This is accomplished using perturbation theory to derive analytic expressions for the electric dipole coupling tensors of perfect planar and rectangular channel reflectors-directly related to a number of important energy transfer processes. In the near field, the separation dependence along the cavity axi… Show more
“…The matrix element for energy pooling has an analogous form to Equation (35); the only difference is that the superscript m0 on A (which is now a donor) becomes 0n and the superscript 00 on M (now the acceptor) becomes s0, where s signifies a doubly excited molecule. In recent years, Lusk et al have demonstrated energy pooling experimentally [146] and discovered, among other advances, that the efficiency of energy pooling can be improved within a cavity [147][148][149]. Lately, moreover, they have studied the time-inverse mechanism of energy pooling, known as quantum cutting, which involves the excitation on A transferring to both D molecules [150].…”
Section: Recent Ret Research Nanomaterials For Energy Transfermentioning
Resonance energy transfer (RET), the transport of electronic energy from one atom or molecule to another, has significant importance to a number of diverse areas of science. Since the pioneering experiments on RET by Cario and Franck in 1922, the theoretical understanding of the process has been continually refined. This review presents a historical account of the post-Förster outlook on RET, based on quantum electrodynamics, up to the present-day viewpoint. It is through this quantum framework that the short-range, R −6 distance dependence of Förster theory was unified with the long-range, radiative transfer governed by the inverse-square law. Crucial to the theoretical knowledge of RET is the electric dipole-electric dipole coupling tensor; we outline its mathematical derivation with a view to explaining some key physical concepts of RET. The higher order interactions that involve magnetic dipoles and electric quadrupoles are also discussed. To conclude, a survey is provided on the latest research, which includes transfer between nanomaterials, enhancement due to surface plasmons, possibilities outside the usual ultraviolet or visible range and RET within a cavity.
“…The matrix element for energy pooling has an analogous form to Equation (35); the only difference is that the superscript m0 on A (which is now a donor) becomes 0n and the superscript 00 on M (now the acceptor) becomes s0, where s signifies a doubly excited molecule. In recent years, Lusk et al have demonstrated energy pooling experimentally [146] and discovered, among other advances, that the efficiency of energy pooling can be improved within a cavity [147][148][149]. Lately, moreover, they have studied the time-inverse mechanism of energy pooling, known as quantum cutting, which involves the excitation on A transferring to both D molecules [150].…”
Section: Recent Ret Research Nanomaterials For Energy Transfermentioning
Resonance energy transfer (RET), the transport of electronic energy from one atom or molecule to another, has significant importance to a number of diverse areas of science. Since the pioneering experiments on RET by Cario and Franck in 1922, the theoretical understanding of the process has been continually refined. This review presents a historical account of the post-Förster outlook on RET, based on quantum electrodynamics, up to the present-day viewpoint. It is through this quantum framework that the short-range, R −6 distance dependence of Förster theory was unified with the long-range, radiative transfer governed by the inverse-square law. Crucial to the theoretical knowledge of RET is the electric dipole-electric dipole coupling tensor; we outline its mathematical derivation with a view to explaining some key physical concepts of RET. The higher order interactions that involve magnetic dipoles and electric quadrupoles are also discussed. To conclude, a survey is provided on the latest research, which includes transfer between nanomaterials, enhancement due to surface plasmons, possibilities outside the usual ultraviolet or visible range and RET within a cavity.
“…Note that there is no space confinement for the propagating direction of the cavity modes, like waveguide modes. A previous study reported that the coupling factors of the cavity modes have 1/ R y dependence when kR y > 1 (far-field regime), and here we show how this evolves into the near field. A similar result is exhibited in the system with the transition dipoles of both the donor and the acceptor aligned along the y direction (Figure S4).…”
Section: Resultsmentioning
confidence: 85%
“…In addition to the RET enhancements along the cavity axis, the cavity modes also influence the RET along the direction parallel to the plane, , which is demonstrated in Figure d–f. Figure d considers the RET enhancement when the acceptor moves along the y direction, with Figure e showing the dependence of EF th on R y for the perfect cavity and Figure f showing that for the silver FP cavity.…”
Long-range
resonance energy transfer (RET) and the control of energy
transfer on the nanoscale have received considerable attention both
experimentally and theoretically during the past few decades. We have
investigated the RET between a donor/acceptor pair in the nanocavities
based on our previous theory developed in the framework of macroscopic
quantum electrodynamics (QED). On the basis of this theory, the enhancements
in the RET with respect to the rate in vacuum were evaluated for a
Fabry–Pérot cavity. When the displacement vector between
the two molecules is aligned with the cavity axis of the Fabry–Pérot
cavity, we find that cavity modes give enhancements of less than a
factor of 10 due to the interference between contributions from resonant
and non-resonant cavity modes. By comparison, when the displacement
vector between the two molecules is aligned in a plane perpendicular
to the cavity axis, we find that the cavity modes can induce enhancements
of more than a factor of 10, and the surface plasmon-polariton modes
can induce enhancements of up to a factor of 300. We develop a convenient
representation for understanding the effect of the displacement vector
between the molecules and of the molecular dipole directions in terms
of the H-dimer and J-dimer properties. To further enhance the RET,
we propose a square silver cavity that gives a rate enhancement of
a factor of 280 under cavity resonance conditions, which provides
important insight into developing devices capable of long-range RET.
“…[29][30][31][32][33][34] However, there are ongoing debates stimulated by modern nanofabrication techniques, about controlling RET purely by means of the nanophotonic environment. Indeed, theory and experiments have revealed both enhanced and inhibited RET rates for many different nanophotonic systems, ranging from plasmonic systems to spasers.…”
The ability to control light-matter interactions in quantum objects opens up many avenues for new applications. We look at this issue within a fully quantized framework using a fundamental theory to describe mirror-assisted resonance energy transfer (RET) in nanostructures. The process of RET communicates electronic excitation between suitably disposed donor and acceptor particles in close proximity, activated by the initial excitation of the donor. Here, we demonstrate that the energy transfer rate can be significantly controlled by careful positioning of the RET emitters near a mirror. The results deliver equations that elicit new insights into the associated modification of virtual photon behavior, based on the quantum nature of light. In particular, our results indicate that energy transfer efficiency in nanostructures can be explicitly expedited or suppressed by a suitably positioned neighboring mirror, depending on the relative spacing and the dimensionality of the nanostructure. Interestingly, the resonance energy transfer between emitters is observed to "switch off" abruptly under suitable conditions of the RET system. This allows one to quantitatively control RET systems in a new way.
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